Art of producing waterproof sheets from fibrous material by the use of sulphur



Patented May 12, 1925.

UNITED STATES 1,531,752 PATENT 'orrlca.

FRANK H. COYNE, OF BRYN MAWR, PENNSYLVANIA; FRANCES MOFIETT COYNE EXECUTRIX O'F SAID FRANK H. COYNE, DECEASED.

ART OF PRODUCING WATERPROOF SHEETS FROM FIBROUS MATERIAL BY THE USE O! SULPHUR.

No Drawing.

To all whom it may concern:

Be it known that I, FRANK H. GoYNE, a citizen of the United States, and a resident of Bryn "Mawr, in the county of Montgomery and State of Pennsylvanla, have invented an Improvement in Art of Producing Waterproof Sheets from Fibrous Material by the Use of Sulphur, of whlch the following is a specification.

My invention has relation to a method of using sulphur as an adhesive in uniting objects or fabrics, and to the composite object or fabric thus produced, with the purpose of giving to such composite ob ects on fabrics or objects produced therefrom, liquid proof and moisture proof and other desirable qualities. My invention also 1ncludes the composite object and fabric thus produced.

This process is particularly applicable to uniting sheets of material, such as sheets of paper, veneer, or other materlals used in building up laminated objects or materials.

I effect the result indicated by introducing my sulphur between the articles or sheets to be united, when the sulphur is in a peculiar condition.

Sulphur occurs crystallized in yellow transparent crystals in the form of rhombic octahedra. It, however, occurs in several physical and molecular forms when subjected to the influence of heat. It becomes thick and viscous, treacly or plastic at temperatures ranging from 320F. to 838 F., when it boils. It is known that if sulphur, when in this thickened condition, be suddenly greatly lowered in temperature, as by pouring asmall stream or film into cold water, or by subjecting a thin film or ribbon-like mass to other sudden chilling effect, it is converted into a soft mass resembling caoutchouc.

This form is not permanent, but after a length of time, depending upon the bulk and other conditions, the sulphur assumes a rigid state. It is at this point that my discovery comes in.

The object of my invention is to produce a more homogeneous product than heretofore, as far as I am aware, has been pro duced, also to produce one which is more nearly completely water-proof than such Application filed March a. 1919. Serial No. 281,465.

products as heretofore manufactured and also to cheapen the cost of production.

I have discovered that under certain conditions as to temperature and method of application, sulphur may be employed as an adhesive for the purpose of securing together two or more sheets of fibrous material to thereby produce a laminated sheet of such material.

My invention has other objects and advantages which will be pointed out in the detailed description thereof which follows or will be apparent from such description.

I have discovered that sulphur, when in a molten state, may be employed as an adhesive to secure together sheets of fibrous or other material. When employing the sulphur as an adhesive, been that it should be raised to a temperature well above its lowest fusion point.

My experience indicates that preferably such temperature should be not less than approximately 300 F.

It is desirable to employ the adhesive (sulphur) when its adhesive quality is at the highest. The adhesive, sulphur, may be used to unite the plies of a composite sheet, applied when in the condition indicated, or the peculiarity in question may be induced by the use of heat after the ap li-' cation of sulphur in powdered or ot er substantially non-adherent condition. The temperature at this point is too high for the fiber to stand long. If the super-melted sulphur be used and distributed in any of the well known ways, it is in condition immediately upon contact with the surface of the sheet to be coated and adheres to it. A. second sheet is immediately and as nearly simultaneously as possible, applied in turn to the sticky adhesive coating so that the two sheets are immediately stuck together by a sticky, tough coherent and temporarily flexible, plastic coating. It may be shaped while in this condition. That is to say the composite sheet, or laminated material, may be bent, or rolled, up etc. according to the flexibility, or pliability, of its constituent sheets other than their interposed layer of, at that stage, plastic, or flexible, sulphur, for example the composite sheet in its thus flexible condition may be shaped from flat into tubular, or cylindrical, contour withmy experience has substances in a viscous, or mobile, liquid I therefore believe that its said condition, then possessing in itself the quality of flexibility, or plastlcity, and, to an extent, also imparting the same to the sheets of other material constitutin the composite, or laminated, article which the sul hur forms a material part.

er the sulphur in in complex product has hardened, or set, its exibihty and plas-' ticity, and,vto a degree, of the article, or laminated composite sheet, of which it forms a part, may, whenever, and as long as above its lowest fusion point and while it is in a viscous or liquid condition, it acts as an eflicient adhesive, articularly in the securing together of rous sheets, but believe'that it may be due to the fact that 70 upon the application of the sulphur atthe relatively high tem erature suggested, it is quickly cooled, an as the temperature is lowered it reaches a point at which the layer of sulphuris in a thorou hly liquid 7 state, in whlch condition it com%)ines with and adheres to the adjacent surfaces of the sheets to be connected. Further cooling to a tem rature belowits lowest fusion int desired for special purposes, be restored, qu ick y takes place so that the layer 0 sulas, for example, by heating to an above phur is hardened and constitutes an eflireferred to temperature and again quickly cooling, thus substantially reutilizing, in that way and'to that extent, a characteristic feature of my above described invention.

Thus, in all cases there is a period, or stage, during which my novel complex sulphurcemented article, or product, is usefull flexible or fplastic, or, after it has hardene capable 0 being again made flexible or lastic, and again relatively rigid or un- Eending by aid of my invention, .and I products, the sulphur of which has hardene or set, are, as well as the therein sulphur, properly definable as being latently plastic, that is to say possessing the r0 erty of becoming indefinitely alternate y. exib le or the reverse without permanent loss, or modification, of their other normal characteristics or qualities.

I do not, however, desire to limit my in- J vention to the use of sulphur at a temperature greater than-300 ,.because it may be found that under some circumstances and conditions it may be practicable to employ it as an adhesive at a substantially ower temperature.

In the employment of sulphur as an adhesive according to my invention, it is placed in a suitable receptacle and raised to a temperature such as above indicated, and by known means is applied to the surface or surfaces of sheets to be secured together. After the sul hur, which may be ma viscous or a mobi e liquid condition, is applied to the surface or surfaces of the sheets to be secured together, such surfaces are placed in contact with each other and are pressed together, The sulphur quickly sets and hardens and constitutes not only an efficient adhesive for connecting the sheets together, but also constitutes a water and moisture proof layer for, preventing the passage of water or moisture through the -aminated sheet formed by the joining together of .two or more sheets.

I have been unable to determine within a degree of certainty why it is that when sulcientbinding agent or adheres as above described.

I claim '1. The process of making a laminated 35 paper structure which consists in moving a layer of paper over a support, applying to said layer, while it is movm over the said support, sulphur previously eated until it reaches a temporarily viscous adhesive condition and while the sulphur is still in its adhesive condition applying a second sheet and subjectin said sheets after sulphur has been app ied and they are stuck together to conditions which transform them into an elastic and temporarily flexible fabric. 7 I

2. As a new article of manufacture, a fabric consisting of layers of material having between them layers of sulphur, thelayers of sulphur procured between said layers of material in adhesive condition, saidfabric being liquid and moisture-proof, and normally stifi' but latently plastic.

3. The new article of manufacture which comprises a plurality of mutually parallel layers or sheets of paper materlal which are held together by a substantially co-extensive, latently plastic, layer or sheet composed essentially of'sul hur interposed beno tween, to an extent com ined with, and adherent to," the respectively mutually op-,. plcsite. areas of first mentioned layers or s eets.

4. The rocess of making a laminated sheet whic consists in procuring between successive layers of paper, layers of sulphur in viscous condition, efi'ecting quick chilling of-said sulphur to adherent condition and a plying pressure to distribute the sulphur tween the sheets and to force it into intimate adherent relation to the fibers of the pa er.

5. T e process which consists in juxtaposing alternate la ers of sulphur heated to viscosity, and 0 organic, fibrous material, chilling the sulphur to adhesive condition, before the fibrous material becomes prohibitively heated, and compressing the no phur is applied at a temperature much layers.

6. The method of uniting sheets of paper material which comprises interposing sulphur in causing it .visoousstate between them and to adhere to the therewith rematerial co mbined together 'by intervening sulphur in the form of a continuous, Water and moisture-proof, layer composed of 00- 10 flllSe mutually co-adherent particles of sulp 1111'.

In testimony that I claim the foregoing as my inventlon I have hereunto set my hand this 27 day of January, A. D., 1919. v FRANK H. COYNE- 

